Dual-region synergistic modulation and (101) facet engineering for highly reversible zinc anodes

作者：Shuai Zhang, Kittima Lolupiman, Dongdong Zhang, Zixuan Gao, Rungroj Chanajaree, Xinyu Zhang, Jin Cao, Jiaqian Qin · 发表于：Advanced Powder Materials · 年份：2025 · DOI：10.1016/j.apmate.2025.100359 · 被引用次数：34 · 研究领域：Advanced battery technologies research、Advanced Battery Technologies Research、Advancements in Battery Materials

Aqueous zinc-ion batteries (AZIBs) offer promising safety and affordability, but suffer from dendritic Zn growth and parasitic side reactions at the electrode-electrolyte interface. Herein, we construct a dual-region interfacial modulation framework by molecularly reconfiguring the Helmholtz double layer via trace methyl methacrylate (MMA). Exploiting its amphiphilic and functionally asymmetric architecture, MMA enables a coordinated interfacial reconstruction that disrupts Zn 2+ solvation in the outer Helmholtz plane, builds a chemisorbed coordination layer in the inner plane, and modulates local interfacial chemistry with spatial precision. This dual-region regulation collectively suppresses water reactivity, facilitates Zn 2+ desolvation, and drives crystallographically preferred deposition along the (101) plane, promoting lateral growth and mitigating dendrite formation. As a result, symmetric Zn||Zn cells exhibit over 4200 hours of stable cycling at 1 mA cm -2 and maintain 1100 hours of operation at 2 mA cm -2 , even at 0 °C. Zn||Ti half-cells achieve a Coulombic efficiency of 99.83%, while Zn||NH 4 V 4 O 10 full cells deliver 93.92% capacity retention after 400 cycles at 2 A g -1 , and preserve 85.3% after 300 cycles at 0 °C. This work demonstrates a scalable, mechanism-driven electrolyte design paradigm for dendrite-free and high-performance aqueous Zn metal batteries. MMA interacts with Zn 2+ in both the outer and inner Helmholtz planes, restructuring the electrolyte ...